Spherical clusters of NiO nanoshafts were prepared using a simple, rapid, and easily scaled up method, i.e., chemical precipitation followed by thermal decomposition. The microstructural characteristics of spherical clusters of nanoshafts were examined by scanning electron microscopy, which showed that the NiO nanoshafts were arranged randomly on the surface of the spherical particles and had grown from the center of the spherical particles to their surface. The electrochemical properties of the assynthesized NiO nanoshaft clusters were investigated to determine their suitability as anode materials for lithium-ion batteries. The nanoshaft cluster electrodes exhibited better reversibility and higher capacities than NiO nanoparticle electrodes. The reasons for the improved electrochemical performance of the nanoshaft cluster electrodes are discussed.